Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)

Yue Zhang; Yuzhi Chen; Andrew T. Lambe; Nicole E. Olson; Ziying Lei; Rebecca L. Craig; Zhenfa Zhang; Avram Gold; Timothy B. Onasch; John T. Jayne; Douglas R. Worsnop; Cassandra J. Gaston; Joel A. Thornton; William Vizuete; Andrew P. Ault; Jason D. Surratt

doi:10.1021/acs.estlett.8b00044

Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)

Yue Zhang, Yuzhi Chen, Andrew T. Lambe, Nicole E. Olson, Ziying Lei, Rebecca L. Craig, Zhenfa Zhang, Avram Gold, Timothy B. Onasch, John T. Jayne, Douglas R. Worsnop, Cassandra J. Gaston, Joel A. Thornton, William Vizuete, Andrew P. Ault, Jason D. Surratt

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150 Scopus citations

Abstract

Acid-catalyzed reactions between gas- and particle-phase constituents are critical to atmospheric secondary organic aerosol (SOA) formation. The aerosol-phase state is thought to influence the reactive uptake of gas-phase precursors to aerosol particles by altering diffusion rates within particles. However, few experimental studies have explored the precise role of the aerosol-phase state on reactive uptake processes. This laboratory study systematically examines the reactive uptake coefficient (γ) of trans-β-isoprene epoxydiol (trans-β-IEPOX), the predominant IEPOX isomer, on acidic sulfate particles coated with SOA derived from α-pinene ozonolysis. γ_IEPOX is obtained for core-shell particles, the morphology of which was confirmed by microscopy, as a function of SOA coating thickness and relative humidity. γ_IEPOX is reduced, in some cases by half of the original value, when SOA coatings are present prior to uptake, especially when coating thicknesses are >15 nm. The diurnal trend of IEPOX lost to acid-catalyzed reactive uptake yielding SOA compared with other known atmospheric sinks (gas-phase oxidation or deposition) is derived by modeling the experimental coating effect with field data from the southeastern United States. IEPOX-derived SOA is estimated to be reduced by 16-27% due to preexisting organic coatings during the afternoon (12:00 to 7:00 p.m., local time), corresponding to the period with the highest level of production.

Original language	English
Pages (from-to)	167-174
Number of pages	8
Journal	Environmental Science and Technology Letters
Volume	5
Issue number	3
DOIs	https://doi.org/10.1021/acs.estlett.8b00044
State	Published - Mar 13 2018

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Zhang, Y., Chen, Y., Lambe, A. T., Olson, N. E., Lei, Z., Craig, R. L., Zhang, Z., Gold, A., Onasch, T. B., Jayne, J. T., Worsnop, D. R., Gaston, C. J., Thornton, J. A., Vizuete, W., Ault, A. P., & Surratt, J. D. (2018). Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX). Environmental Science and Technology Letters, 5(3), 167-174. https://doi.org/10.1021/acs.estlett.8b00044

@article{3e2c05ccf86c4eb68bf35c321dacdc98,

title = "Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)",

abstract = "Acid-catalyzed reactions between gas- and particle-phase constituents are critical to atmospheric secondary organic aerosol (SOA) formation. The aerosol-phase state is thought to influence the reactive uptake of gas-phase precursors to aerosol particles by altering diffusion rates within particles. However, few experimental studies have explored the precise role of the aerosol-phase state on reactive uptake processes. This laboratory study systematically examines the reactive uptake coefficient (γ) of trans-β-isoprene epoxydiol (trans-β-IEPOX), the predominant IEPOX isomer, on acidic sulfate particles coated with SOA derived from α-pinene ozonolysis. γIEPOX is obtained for core-shell particles, the morphology of which was confirmed by microscopy, as a function of SOA coating thickness and relative humidity. γIEPOX is reduced, in some cases by half of the original value, when SOA coatings are present prior to uptake, especially when coating thicknesses are >15 nm. The diurnal trend of IEPOX lost to acid-catalyzed reactive uptake yielding SOA compared with other known atmospheric sinks (gas-phase oxidation or deposition) is derived by modeling the experimental coating effect with field data from the southeastern United States. IEPOX-derived SOA is estimated to be reduced by 16-27\% due to preexisting organic coatings during the afternoon (12:00 to 7:00 p.m., local time), corresponding to the period with the highest level of production.",

author = "Yue Zhang and Yuzhi Chen and Lambe, \{Andrew T.\} and Olson, \{Nicole E.\} and Ziying Lei and Craig, \{Rebecca L.\} and Zhenfa Zhang and Avram Gold and Onasch, \{Timothy B.\} and Jayne, \{John T.\} and Worsnop, \{Douglas R.\} and Gaston, \{Cassandra J.\} and Thornton, \{Joel A.\} and William Vizuete and Ault, \{Andrew P.\} and Surratt, \{Jason D.\}",

note = "Publisher Copyright: {\textcopyright} 2018 American Chemical Society.",

year = "2018",

month = mar,

day = "13",

doi = "10.1021/acs.estlett.8b00044",

language = "English",

volume = "5",

pages = "167--174",

journal = "Environmental Science and Technology Letters",

issn = "2328-8930",

publisher = "American Chemical Society",

number = "3",

}

Zhang, Y, Chen, Y, Lambe, AT, Olson, NE, Lei, Z, Craig, RL, Zhang, Z, Gold, A, Onasch, TB, Jayne, JT, Worsnop, DR, Gaston, CJ, Thornton, JA, Vizuete, W, Ault, AP & Surratt, JD 2018, 'Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)', Environmental Science and Technology Letters, vol. 5, no. 3, pp. 167-174. https://doi.org/10.1021/acs.estlett.8b00044

TY - JOUR

T1 - Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)

AU - Zhang, Yue

AU - Chen, Yuzhi

AU - Lambe, Andrew T.

AU - Olson, Nicole E.

AU - Lei, Ziying

AU - Craig, Rebecca L.

AU - Zhang, Zhenfa

AU - Gold, Avram

AU - Onasch, Timothy B.

AU - Jayne, John T.

AU - Worsnop, Douglas R.

AU - Gaston, Cassandra J.

AU - Thornton, Joel A.

AU - Vizuete, William

AU - Ault, Andrew P.

AU - Surratt, Jason D.

PY - 2018/3/13

Y1 - 2018/3/13

N2 - Acid-catalyzed reactions between gas- and particle-phase constituents are critical to atmospheric secondary organic aerosol (SOA) formation. The aerosol-phase state is thought to influence the reactive uptake of gas-phase precursors to aerosol particles by altering diffusion rates within particles. However, few experimental studies have explored the precise role of the aerosol-phase state on reactive uptake processes. This laboratory study systematically examines the reactive uptake coefficient (γ) of trans-β-isoprene epoxydiol (trans-β-IEPOX), the predominant IEPOX isomer, on acidic sulfate particles coated with SOA derived from α-pinene ozonolysis. γIEPOX is obtained for core-shell particles, the morphology of which was confirmed by microscopy, as a function of SOA coating thickness and relative humidity. γIEPOX is reduced, in some cases by half of the original value, when SOA coatings are present prior to uptake, especially when coating thicknesses are >15 nm. The diurnal trend of IEPOX lost to acid-catalyzed reactive uptake yielding SOA compared with other known atmospheric sinks (gas-phase oxidation or deposition) is derived by modeling the experimental coating effect with field data from the southeastern United States. IEPOX-derived SOA is estimated to be reduced by 16-27% due to preexisting organic coatings during the afternoon (12:00 to 7:00 p.m., local time), corresponding to the period with the highest level of production.

AB - Acid-catalyzed reactions between gas- and particle-phase constituents are critical to atmospheric secondary organic aerosol (SOA) formation. The aerosol-phase state is thought to influence the reactive uptake of gas-phase precursors to aerosol particles by altering diffusion rates within particles. However, few experimental studies have explored the precise role of the aerosol-phase state on reactive uptake processes. This laboratory study systematically examines the reactive uptake coefficient (γ) of trans-β-isoprene epoxydiol (trans-β-IEPOX), the predominant IEPOX isomer, on acidic sulfate particles coated with SOA derived from α-pinene ozonolysis. γIEPOX is obtained for core-shell particles, the morphology of which was confirmed by microscopy, as a function of SOA coating thickness and relative humidity. γIEPOX is reduced, in some cases by half of the original value, when SOA coatings are present prior to uptake, especially when coating thicknesses are >15 nm. The diurnal trend of IEPOX lost to acid-catalyzed reactive uptake yielding SOA compared with other known atmospheric sinks (gas-phase oxidation or deposition) is derived by modeling the experimental coating effect with field data from the southeastern United States. IEPOX-derived SOA is estimated to be reduced by 16-27% due to preexisting organic coatings during the afternoon (12:00 to 7:00 p.m., local time), corresponding to the period with the highest level of production.

UR - https://www.scopus.com/pages/publications/85043781097

U2 - 10.1021/acs.estlett.8b00044

DO - 10.1021/acs.estlett.8b00044

M3 - Article

AN - SCOPUS:85043781097

SN - 2328-8930

VL - 5

SP - 167

EP - 174

JO - Environmental Science and Technology Letters

JF - Environmental Science and Technology Letters

IS - 3

ER -

Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)

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